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Ba3Yb2Zn5O11 is unique among breathing pyrochlore compounds for being in thenearly decoupled limit where inter-tetrahedron interactions are weak, hostingisolated clusters or "molecular magnet" like tetrahedra of magnetic ytterbium(Yb3+) ions. In this work, we present the first study carried out onsingle-crystal samples of the breathing pyrochlore Ba3Yb2Zn5O11, using avariety of magnetometry and neutron scattering techniques along withtheoretical modeling. We employ inelastic neutron scattering to investigate themagnetic dynamics as a function of applied field (with respect to bothmagnitude and direction) down to a temperature of 70 mK, where inelasticscattering reveals dispersionless bands of excitations as found in earlierpowder sample studies, in good agreement with a single-tetrahedron model.However, diffuse neutron scattering at zero field and dc-susceptibility atfinite field exhibit features suggesting the presence of excitations atlow-energy that are not captured by the single tetrahedron model. Analysis ofthe local structure down to 2 K via pair distribution function analysis findsno evidence of structural disorder. We conclude that effects beyond the singletetrahedron model are important in describing the low-energy, low temperaturephysics of Ba3Yb2Zn5O11, but their nature remains undetermined.

Towards understanding the magnetic properties of the breathing pyrochlore compound Ba3Yb2Zn5O11: A single crystal study